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Supramolecular polymers form tactoids through liquid–liquid phase separation

Author

Listed:
  • Hailin Fu

    (Eindhoven University of Technology
    Eindhoven University of Technology)

  • Jingyi Huang

    (Eindhoven University of Technology
    Eindhoven University of Technology)

  • Joost J. B. van der Tol

    (Eindhoven University of Technology
    Eindhoven University of Technology)

  • Lu Su

    (Leiden University)

  • Yuyang Wang

    (Eindhoven University of Technology
    Eindhoven University of Technology)

  • Swayandipta Dey

    (Eindhoven University of Technology
    Eindhoven University of Technology
    Eindhoven University of Technology)

  • Peter Zijlstra

    (Eindhoven University of Technology
    Eindhoven University of Technology
    Eindhoven University of Technology)

  • George Fytas

    (Eindhoven University of Technology
    Max Planck Institute for Polymer Research
    Institute of Electronic Structure and Laser, FO.R.T.H)

  • Ghislaine Vantomme

    (Eindhoven University of Technology
    Eindhoven University of Technology)

  • Patricia Y. W. Dankers

    (Eindhoven University of Technology
    Eindhoven University of Technology)

  • E. W. Meijer

    (Eindhoven University of Technology
    Eindhoven University of Technology
    University of New South Wales)

Abstract

Liquid–liquid phase separation (LLPS) of biopolymers has recently been shown to play a central role in the formation of membraneless organelles with a multitude of biological functions1–3. The interplay between LLPS and macromolecular condensation is part of continuing studies4,5. Synthetic supramolecular polymers are the non-covalent equivalent of macromolecules but they are not reported to undergo LLPS yet. Here we show that continuously growing fibrils, obtained from supramolecular polymerizations of synthetic components, are responsible for phase separation into highly anisotropic aqueous liquid droplets (tactoids) by means of an entropy-driven pathway. The crowding environment, regulated by dextran concentration, affects not only the kinetics of supramolecular polymerizations but also the properties of LLPS, including phase-separation kinetics, morphology, internal order, fluidity and mechanical properties of the final tactoids. In addition, substrate–liquid and liquid–liquid interfaces proved capable of accelerating LLPS of supramolecular polymers, allowing the generation of a myriad of three-dimensional-ordered structures, including highly ordered arrays of micrometre-long tactoids at surfaces. The generality and many possibilities of supramolecular polymerizations to control emerging morphologies are demonstrated with several supramolecular polymers, opening up a new field of matter ranging from highly structured aqueous solutions by means of stabilized LLPS to nanoscopic soft matter.

Suggested Citation

  • Hailin Fu & Jingyi Huang & Joost J. B. van der Tol & Lu Su & Yuyang Wang & Swayandipta Dey & Peter Zijlstra & George Fytas & Ghislaine Vantomme & Patricia Y. W. Dankers & E. W. Meijer, 2024. "Supramolecular polymers form tactoids through liquid–liquid phase separation," Nature, Nature, vol. 626(8001), pages 1011-1018, February.
  • Handle: RePEc:nat:nature:v:626:y:2024:i:8001:d:10.1038_s41586-024-07034-7
    DOI: 10.1038/s41586-024-07034-7
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    Cited by:

    1. Hongni Chen & Chao Wang & Han Wu & Lili Li & Yali Xing & Chuanhui Zhang & Xiaojing Long, 2024. "Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-14, December.

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